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An Ambient Measurement Technique for Vehicle Emission Quantification and Concentration Source Apportionment. 用于车辆排放定量和浓度源分配的环境测量技术。
IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-12 Epub Date: 2024-11-03 DOI: 10.1021/acs.est.4c07907
Naomi J Farren, Samuel Wilson, Yoann Bernard, Marvin D Shaw, Kaylin Lee, Mallery Crowe, David C Carslaw

We develop a new technique called plume regression where fast response instruments located at the roadside are used to measure exhaust plumes of passing vehicles. The approach is used to generate highly disaggregated vehicle emissions information by vehicle type, which compares well with traditional vehicle emission remote sensing. Additionally, the technique provides valuable new information on ambient concentration source apportionment by vehicle type. The technique is flexible enough to consider a wide range of air pollutants and be deployed at roadside ambient monitoring locations. The new approach is used to quantify emissions and concentration source apportionment for ammonia (NH3) and nitrogen oxides (NOx). We find that emissions of NH3 are generally very well controlled from diesel vehicles including those with selective catalytic reduction systems that use NH3 to reduce emissions of NOx. By contrast, gasoline passenger cars are shown to be the dominant contributor to NH3 emissions, which increase with vehicle mileage. Average fuel-specific NH3 emission factors for gasoline vehicles range from 0.3 to 1.2 g kg-1, while diesel vehicle emission factors remain below 0.06 g kg-1, with the exception of Euro VI buses with the latest regulatory provisions (0.5 g kg-1).

我们开发了一种名为 "羽流回归 "的新技术,利用路边的快速反应仪器测量过往车辆的尾气羽流。这种方法可用于生成按车辆类型高度分类的车辆排放信息,与传统的车辆排放遥感技术相比效果更佳。此外,该技术还为按车辆类型划分环境浓度源提供了宝贵的新信息。该技术非常灵活,可以考虑多种空气污染物,并可部署在路边环境监测点。新方法用于量化氨(NH3)和氮氧化物(NOx)的排放量和浓度源分配。我们发现,NH3 的排放一般都能得到很好的控制,包括那些装有选择性催化还原系统的柴油车,该系统使用 NH3 来减少氮氧化物的排放。相比之下,汽油乘用车是 NH3 排放的主要来源,其排放量随着汽车行驶里程的增加而增加。汽油车的特定燃料 NH3 平均排放系数介于 0.3 至 1.2 克/千克之间,而柴油车的排放系数则保持在 0.06 克/千克以下,但符合最新法规规定(0.5 克/千克)的欧 VI 巴士除外。
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引用次数: 0
Enzymatic Degradation toward Herbicides: The Case of the Sulfonylureas. 除草剂的酶降解:磺酰脲类的案例。
IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-12 Epub Date: 2024-10-01 DOI: 10.1021/acs.est.4c04929
Mingna Zheng, Yanwei Li, Qingzhu Zhang, Wenxing Wang

Commercial herbicides, particularly sulfonylureas, are used worldwide and pose a significant challenge to environmental sustainability. The efficient degradation of sulfonylurea herbicides is critical. SulE, an esterase isolated from the bacterial strain Hansschlegelia zhihuaiae S113, shows degradation activity toward sulfonylurea herbicides. However, the detailed catalytic mechanism remains vague to a large extent. Herein, we decipher the SulEP44R-catalyzed degradation mechanism of sulfonylurea herbicides using hybrid quantum mechanics and molecular mechanics approaches. Our results show that the degradation of sulfonylureas catalyzed by SulEP44R involves four concerted elementary steps. The rate-determining step has an energy barrier range of 19.7-21.4 kcal·mol-1, consistent with the experimentally determined range of 16.0-18.0 kcal·mol-1. Distortion/interaction analysis demonstrates that active-site amino acids play a vital role in the enzymatic catalytic efficacy. The unique architecture of SulEP44R's active site can serve as an excellent template for designing artificial catalysts. Key structural and charge parameters affecting catalytic activity were systematically screened and identified. Based on the elucidated degradation mechanism, several new herbicides with both high herbicidal activity and biodegradability were developed with the aid of a high-throughput strategy. Our findings may advance the application of sulfonylurea herbicides within the framework of environmental sustainability.

商用除草剂,尤其是磺酰脲类除草剂,在全球范围内广泛使用,对环境的可持续发展构成了重大挑战。高效降解磺酰脲类除草剂至关重要。SulE 是一种从细菌菌株 Hansschlegelia zhihuaiae S113 中分离出来的酯酶,具有降解磺酰脲类除草剂的活性。然而,详细的催化机理在很大程度上仍然模糊不清。在此,我们利用量子力学和分子力学的混合方法破译了 SulEP44R 催化磺酰脲类除草剂的降解机制。我们的研究结果表明,SulEP44R 催化的磺酰脲类除草剂降解过程涉及四个协同的基本步骤。速率决定步骤的能障范围为 19.7-21.4 kcal-mol-1,与实验测定的 16.0-18.0 kcal-mol-1 范围一致。畸变/相互作用分析表明,活性位点氨基酸对酶的催化效率起着至关重要的作用。SulEP44R 活性位点的独特结构可作为设计人工催化剂的绝佳模板。我们系统地筛选并鉴定了影响催化活性的关键结构和电荷参数。在阐明降解机理的基础上,利用高通量策略开发出了几种具有高除草活性和生物降解性的新型除草剂。我们的发现可能会推动磺酰脲类除草剂在环境可持续发展框架内的应用。
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引用次数: 0
The Universal Neighborhood Effect Averaging in Mobility-Dependent Environmental Exposures. 依赖流动性的环境暴露中的通用邻里效应平均化。
IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-12 Epub Date: 2024-10-03 DOI: 10.1021/acs.est.4c02464
Jiannan Cai, Mei-Po Kwan

The neighborhood effect averaging problem (NEAP) is a fundamental statistical phenomenon in mobility-dependent environmental exposures. It suggests that individual environmental exposures tend toward the average exposure in the study area when considering human mobility. However, the universality of the NEAP across various environmental exposures and the mechanisms underlying its occurrence remain unclear. Here, using a large human mobility data set of more than 27 000 individuals in the Chicago Metropolitan Area, we provide robust evidence of the existence of the NEAP in a range of individual environmental exposures, including green spaces, air pollution, healthy food environments, transit accessibility, and crime rates. We also unveil the social and spatial disparities in the NEAP's influence on individual environmental exposure estimates. To further reveal the mechanisms behind the NEAP, we perform multiscenario analyses based on environmental variation and human mobility simulations. The results reveal that the NEAP is a statistical phenomenon of regression to the mean (RTM) under the constraints of spatial autocorrelation in environmental data. Increasing travel distances and out-of-home durations can intensify and promote the NEAP's impact, particularly for highly dynamic environmental factors like air pollution. These findings illuminate the complex interplay between human mobility and environmental factors, guiding more effective public health interventions.

邻近效应平均问题(NEAP)是依赖流动性的环境暴露中的一种基本统计现象。它表明,当考虑到人类的流动性时,个体的环境暴露会趋向于研究区域的平均暴露。然而,NEAP 在各种环境暴露中的普遍性及其发生机制仍不清楚。在此,我们利用芝加哥大都会区 27000 多人的大型人口流动数据集,提供了强有力的证据,证明在一系列个体环境暴露中存在 NEAP,包括绿地、空气污染、健康食品环境、交通可达性和犯罪率。我们还揭示了 NEAP 对个体环境暴露估计值影响的社会和空间差异。为了进一步揭示 NEAP 背后的机制,我们基于环境变化和人类流动性模拟进行了多情景分析。结果表明,在环境数据空间自相关性的约束下,NEAP 是一种向均值回归(RTM)的统计现象。旅行距离和离家时间的增加会加剧和促进 NEAP 的影响,特别是对于空气污染等高度动态的环境因素。这些发现揭示了人类流动性与环境因素之间复杂的相互作用,为更有效的公共卫生干预提供了指导。
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引用次数: 0
Two-Dimensional Layered Nano-MoS2 Induces Earthworm Immune Cell Apoptosis by Regulating Lysosomal Maintenance and Function: Toward Unbiased Screening and Validation of Suspicious Pathways. 二维层状纳米 MoS2 通过调节溶酶体的维持和功能诱导蚯蚓免疫细胞凋亡:实现无偏见筛选和验证可疑途径。
IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-12 Epub Date: 2024-10-03 DOI: 10.1021/acs.est.4c04512
Kailun Sun, Cornelis A M van Gestel, Hao Qiu

Molybdenum-based nanosheets (NSMoS2) are increasingly applied in various fields and undergoing relevant risk evaluations on subjectively hypothesized toxicity pathways. However, risk assessment should be unbiased and focus on appropriate end points to avoid biased prescreening. Here, we developed an adverse biological outcome screening strategy based on nontargeted functional protein profiles in earthworm (Eisenia fetida) immune cells exposed to NSMoS2 and their ionic counterpart (Na2MoO4). Through this framework, the apoptosis-related processes with distinct mechanisms were rapidly identified and thoroughly validated phenotypically. Specifically, upon exposure to 50 μg Mo/mL Na2MoO4, cellular signaling and energy homeostasis were disrupted within the transcription-translation biological chain. The autophagic pathway was activated, which, together with energy deprivation, phenotypically induced significant autophagy that ultimately led to apoptosis. In contrast, NSMoS2, tested at the same concentration, caused a reprogramming of apoptotic gene and protein expressions. Transcriptome plasticity facilitated the endocytic-adaptive transcriptional profile characterized by cytoskeleton remodeling and lysosome organization/movement under NSMoS2 exposure. Subcellular dynamics further revealed NSMoS2-induced lysosomal damage with a time-sensitive physiological window, ultimately mediating apoptosis. These findings provide a mechanistic and visual understanding of the distinct risk profile of NSMoS2 compared to molybdate, highlighting the importance of integrating nontargeted screening and phenotypic validation in early risk warning.

钼基纳米片(NSMoS2)越来越多地应用于各个领域,并根据主观臆断的毒性途径进行相关的风险评估。然而,风险评估应不偏不倚,重点关注适当的终点,以避免预筛选出现偏差。在此,我们基于暴露于 NSMoS2 及其离子对应物(Na2MoO4)的蚯蚓(Eisenia fetida)免疫细胞的非靶向功能蛋白图谱,开发了一种不良生物学结果筛选策略。通过这一框架,我们迅速确定了具有不同机制的凋亡相关过程,并从表型上进行了彻底验证。具体来说,暴露于 50 μg Mo/mL Na2MoO4 后,转录-翻译生物链中的细胞信号传导和能量平衡被破坏。自噬途径被激活,再加上能量匮乏,在表型上诱发了显著的自噬,最终导致细胞凋亡。与此相反,在相同浓度下测试的 NSMoS2 会导致凋亡基因和蛋白质表达的重新编程。转录组的可塑性促进了以细胞骨架重塑和溶酶体组织/移动为特征的内吞适应性转录特征。亚细胞动力学进一步揭示了NSMoS2诱导的溶酶体损伤具有时间敏感的生理窗口,最终介导了细胞凋亡。这些发现从机理和视觉上揭示了 NSMoS2 与钼酸盐相比所具有的不同风险特征,突出了在早期风险预警中整合非靶向筛选和表型验证的重要性。
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引用次数: 0
Environmental Machine Learning, Baseline Reporting, and Comprehensive Evaluation: The EMBRACE Checklist. 环境机器学习、基线报告和综合评估:EMBRACE 核对表。
IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-12 Epub Date: 2024-10-29 DOI: 10.1021/acs.est.4c09611
Jun-Jie Zhu, Alexandria B Boehm, Zhiyong Jason Ren
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引用次数: 0
Heavy-Metal Ions Control on PFAS Adsorption on Goethite in Aquatic Systems. 重金属离子对水生系统中鹅卵石吸附全氟辛烷磺酸的控制。
IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-12 Epub Date: 2024-10-31 DOI: 10.1021/acs.est.4c10068
Aaifa Chaudhary, Muhammad Usman, Wei Cheng, Stefan Haderlein, Jean-François Boily, Khalil Hanna

Per- and polyfluoroalkyl substances (PFAS) are ubiquitous environmental contaminants that often co-occur with heavy metals. Despite their prevalence, the mobility of PFAS in complex, multicomponent systems, particularly at the molecular scale, remains poorly understood. The vast diversity of PFAS and their low concentrations alongside anthropogenic and natural substances underscore the need for integrating mechanistic insights into the sorption models. This study explores the influence of metal cations (Cu(II), Cd(II), and Fe(II)) on the adsorption of four common PFAS (PFOA, PFOS, PFDA, and GenX) onto goethite (α-FeOOH), a common iron (oxyhydr)oxide in both aquatic and terrestrial environments. PFAS adsorption was highly dependent on the PFAS type, pH, and metal ion concentration, with a surface complexation model effectively predicting these interactions. Cu(II) and Cd(II) enhanced PFOS and PFDA adsorption via ternary complexation while slightly reducing PFOA and GenX adsorption. Under anoxic conditions, Fe(II) significantly increased the adsorption of all PFAS, showing reactivity greater than those of Cu(II) and Cd(II). Additionally, natural organic matter increased PFAS mobility, although metal cations in groundwater may counteract this by enhancing PFAS retention. These findings highlight the key role of metal cations in PFAS transport and offer critical insights for predicting PFAS behavior at oxic-anoxic environmental interfaces.

全氟和多氟烷基物质(PFAS)是无处不在的环境污染物,经常与重金属共存。尽管 PFAS 非常普遍,但人们对其在复杂、多组分系统中的流动性,尤其是分子尺度的流动性,仍然知之甚少。全氟辛烷磺酸种类繁多,而且与人为物质和天然物质一起存在的浓度很低,这突出表明有必要将机理观点纳入吸附模型。本研究探讨了金属阳离子(Cu(II)、Cd(II) 和 Fe(II))对四种常见全氟辛烷磺酸(PFOA、PFOS、PFDA 和 GenX)在水生和陆生环境中常见的氧化铁(α-FeOOH)上的吸附作用的影响。PFAS 吸附与 PFAS 类型、pH 值和金属离子浓度高度相关,表面络合模型可有效预测这些相互作用。铜(II)和镉(II)通过三元络合增强了对全氟辛烷磺酸和全氟辛烷磺酸的吸附,同时略微降低了对全氟辛酸和玄武岩酸的吸附。在缺氧条件下,Fe(II) 显著增加了对所有 PFAS 的吸附,其反应活性高于 Cu(II) 和 Cd(II)。此外,天然有机物增加了全氟辛烷磺酸的流动性,但地下水中的金属阳离子可能会通过增强全氟辛烷磺酸的滞留来抵消这一作用。这些发现强调了金属阳离子在全氟辛烷磺酸迁移中的关键作用,并为预测全氟辛烷磺酸在缺氧-缺氧环境界面的行为提供了重要见解。
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引用次数: 0
Variability of Biodegradation Rates of Commercial Chemicals in Rivers in Different Regions of Europe. 欧洲不同地区河流中商业化学品生物降解率的变化。
IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-12 Epub Date: 2024-10-28 DOI: 10.1021/acs.est.4c07410
Run Tian, Malte Posselt, Kathrin Fenner, Michael S McLachlan

Biodegradation is one of the most important processes influencing the fate of organic contaminants in the environment. Quantitative understanding of the spatial variability in environmental biodegradation is still largely uncharted territory. Here, we conducted modified OECD 309 tests to determine first-order biodegradation rate constants for 97 compounds in 18 freshwater river segments in five European countries: Sweden, Germany, Switzerland, Spain, and Greece. All but two of the compounds showed significant spatial variability in rate constants across European rivers (ANOVA, P < 0.05). The median standard deviation of the biodegradation rate constant between rivers was a factor of 3. The spatial variability was similar between pristine and contaminated river segments. The longitude, total organic carbon, and clay content of sediment were the three most significant explanatory variables for the spatial variability (redundancy analysis, P < 0.05). Similarities in the spatial pattern of biodegradation rates were observed for some groups of compounds sharing a given functional group. The pronounced spatial variability presents challenges for the use of biodegradation simulation tests to assess chemical persistence. To reflect the variability in the biodegradation rate, the modified OECD 309 test would have to be repeated with water and sediment from multiple sites.

生物降解是影响环境中有机污染物归宿的最重要过程之一。定量了解环境生物降解的空间变异性在很大程度上仍是一个未知领域。在此,我们进行了修改后的 OECD 309 试验,以确定欧洲五国 18 个淡水河段中 97 种化合物的一阶生物降解速率常数:瑞典、德国、瑞士、西班牙和希腊。除两种化合物外,其他所有化合物的降解速率常数在欧洲河流中都存在显著的空间差异(方差分析,P < 0.05)。河流间生物降解速率常数的中位标准偏差为 3 倍,原始河段和受污染河段的空间变异性相似。经度、总有机碳和沉积物的粘土含量是对空间变异性最有意义的三个解释变量(冗余分析,P < 0.05)。在生物降解率的空间模式中,一些同属一个功能群的化合物组具有相似性。明显的空间变异性给使用生物降解模拟试验评估化学品持久性带来了挑战。为了反映生物降解速率的变化,必须用多个地点的水和沉积物重复经修改的 OECD 309 试验。
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引用次数: 0
Waste Nitrogen Upcycling to Amino Acids during Anaerobic Fermentation on Biochar: An Active Strategy for Regulating Metabolic Reducing Power. 生物炭厌氧发酵过程中的废氮转化为氨基酸:调节代谢还原力的主动策略。
IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-12 Epub Date: 2024-11-01 DOI: 10.1021/acs.est.4c08890
Yanfei Tang, Eakalak Khan, Daniel C W Tsang

This study proposes a novel strategy that utilizes biochar (BC) during anaerobic fermentation (AF) to generate amino acids (AAs) toward nitrogen upcycling. The BC, pyrolyzed at 800 °C (BC800) to enhance graphite structures and electron-accepting sites, effectively addresses issues related to biosynthetic reducing power nicotinamide adenine dinucleotide phosphate insufficiency by altering cellular conditions and alleviates feedback inhibition through the immobilization of end products. This process establishes unique microbial signaling and energy networks, with Escherichia coli becoming dominant in the biofilm. The conversion rate of ammonia-N to AAs-N within the biofilm reached 67.4% in BC800-AF, which was significantly higher compared to the levels in other AF reactors with BC pyrolyzed at 600 and 400 °C (45.9 and 22.5%, respectively), as well as a control AF reactor (<5%). Furthermore, in BC800-AF, the aromatic AAs (Aro-AAs) were as high as 70.8% of the AAs within the biofilm. The activities of key enzymes for Aro-AAs biosynthesis uniquely positively correlated with the electron-accepting capacity on BC800 (R2 ≥ 0.95). These findings hold promise for transforming existing AF reactors into factories that produce BC-based AAs, providing a more sustainable fertilizing agent than chemical fertilizers.

本研究提出了一种新策略,即在厌氧发酵(AF)过程中利用生物炭(BC)生成氨基酸(AAs),实现氮的上循环。生物炭在 800 °C(BC800)高温下热解以增强石墨结构和电子接受位点,通过改变细胞条件有效解决了与生物合成还原力烟酰胺腺嘌呤二核苷酸磷酸酯不足有关的问题,并通过固定最终产物缓解了反馈抑制。这一过程建立了独特的微生物信号和能量网络,大肠杆菌在生物膜中占据主导地位。在 BC800-AF 中,生物膜内氨-N 向 AAs-N 的转化率达到 67.4%,与其他在 600 和 400 °C 下热解 BC 的 AF 反应器(分别为 45.9% 和 22.5%)以及对照 AF 反应器(R2 ≥ 0.95)的水平相比显著提高。这些研究结果有望将现有的 AF 反应器改造成生产基于 BC 的 AA 的工厂,提供比化肥更可持续的肥料。
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引用次数: 0
Electric Demulsification Membrane Technology for Confined Separation of Oil-Water Emulsions. 用于油水乳状液密闭分离的电破乳膜技术。
IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-12 Epub Date: 2024-10-29 DOI: 10.1021/acs.est.4c06566
Yuna Gu, Qiancheng Xia, Bin Liu, Yang Zhao, Liangtao Pu, Jie Ding, Yanbiao Liu, Enze Li, Chad D Vecitis, Guandao Gao

Demulsification technology for separation of oil-water (O/W) emulsions, especially those stabilized by surfactants, is urgently needed yet remains highly challenging due to their inherent stability characteristics. Electrocoalescence has emerged as a promising solution owing to its simplicity, efficacy, and versatility, yet hindered by substantial energy consumption (e.g., >50 kWh/m3) along with undesirable Faradic reactions. Herein, we propose an innovative electric demulsification technology that leverages conductive membrane microchannels to confine oil droplets from the oil-water emulsion for achieving high energy-efficient coalescence of oil droplets. The proposed system reduces the required voltage down to 12 V, 2 orders of magnitude lower than that of conventional electrocoalescence systems, while achieving a similar separation efficacy of 91.4 ± 3.0% at a low energy consumption (3 kWh/m3) and an ultrahigh permeability >3000 L/(m2·h·bar). In situ fluorescence microscopy combined with COMSOL simulations provided insight into the fundamental mechanistic steps of an electric demulsification process confined to membrane microchannels: (1) rapid electric-field redistribution of oil droplet surfactant molecules, (2) enhanced collision probability due to confined oil droplet concentration under dielectrophoretic forces, and (3) increased collision efficacy facilitated by the membrane pore structure. This strategy may revolutionize the next generation of demulsification and oil-water separation innovations.

油水(O/W)乳液,尤其是由表面活性剂稳定的油水乳液,急需分离破乳技术,但由于其固有的稳定性特点,这种技术仍然极具挑战性。电凝聚技术因其简单、高效和多功能性而成为一种有前途的解决方案,但其巨大的能耗(例如大于 50 kWh/m3)以及不理想的法拉第反应阻碍了它的发展。在此,我们提出了一种创新的电去乳化技术,利用导电膜微通道来限制油水乳化液中的油滴,从而实现高能效的油滴凝聚。该系统将所需电压降至 12 V,比传统电凝聚系统低 2 个数量级,同时在低能耗(3 kWh/m3)和渗透率大于 3000 L/(m2-h-bar)的超高渗透率条件下实现了 91.4 ± 3.0% 的相似分离效率。原位荧光显微镜与 COMSOL 模拟相结合,使人们深入了解了局限于膜微通道的电破乳过程的基本机理步骤:(1) 油滴表面活性剂分子的快速电场再分布,(2) 在介电泳力作用下,局限的油滴浓度提高了碰撞概率,(3) 膜孔结构提高了碰撞效率。这种策略可能会彻底改变下一代破乳化和油水分离创新技术。
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引用次数: 0
Elucidating Phosphate and Cadmium Cosorption Mechanisms on Mineral Surfaces with Direct Spectroscopic and Modeling Evidence. 利用直接光谱和模型证据阐明矿物表面的磷酸盐和镉共吸附机制
IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-12 Epub Date: 2024-10-31 DOI: 10.1021/acs.est.4c08847
Wantong Zhao, Yun Xu, Liting Gu, Mengqiang Zhu, Peng Yang, Chunhao Gu, Zhe Liu, Xionghan Feng, Wenfeng Tan, Qiaoyun Huang, Xiaoming Wang

The simultaneous sorption of cations and anions at the mineral-water interface can substantially alter their individual sorption characteristics; however, this phenomenon lacks a mechanistic understanding. Our study provides direct spectroscopic and modeling evidence of the molecular cosorption mechanisms of the cadmium ion (Cd2+) and phosphate (P) on goethite and layered manganese (Mn) oxide of birnessite, through in situ attenuated total reflection Fourier-transform infrared (ATR-FTIR), P K-edge X-ray absorption near-edge structure (XANES) spectroscopy, and surface complexation modeling. Phosphate synergistically cosorbed with Cd on goethite predominantly through P-bridged ternary complexes (≡Fe-P-Cd) and electrostatic interactions at wide pH conditions. Likewise, P and Cd exhibited synergistic cosorption on birnessite by forming P-bridged ternary complexes (≡Mn-P-Cd) and weak competitive sorption at the layer edge sites. As pH and Cd loading increased, the surface P species transitioned from a binary complex to a ternary complex and/or Cd3(PO4)2 precipitate for both goethite and birnessite. Compared to that in solution at pH 8, the formation of Cd3(PO4)2 was inhibited by the presence of goethite and birnessite, ascribed to the specific adsorption of P and Cd, more pronounced in birnessite due to the stronger sorption of Cd at its vacant sites. The discovered cosorption mechanisms of P and Cd have important implications for understanding and predicting their mobility and availability in Cd-contaminated settings.

阳离子和阴离子在矿物-水界面上的同时吸附会大大改变它们各自的吸附特性;然而,人们对这一现象缺乏机理上的认识。我们的研究通过原位衰减全反射傅立叶变换红外光谱(ATR-FTIR)、磷矿石 K 边 X 射线吸收近边结构(XANES)光谱和表面络合模型,提供了镉离子(Cd2+)和磷矿石(P)在鹅绿泥石和层状氧化锰(Mn)的分子协同吸附机制的直接光谱和模型证据。在较宽的 pH 值条件下,磷酸盐主要通过 P 桥接三元络合物(≡Fe-P-Cd)和静电作用与镉协同吸附在鹅卵石上。同样,钯和镉通过形成钯桥接三元络合物(≡锰-钯-镉)以及在层边缘位点的弱竞争吸附作用,在桦锰矿上表现出协同共吸附作用。随着 pH 值和镉负载量的增加,鹅绿泥石和桦褐铁矿的表面 P 物种都从二元络合物转变为三元络合物和/或 Cd3(PO4)2 沉淀。与 pH 值为 8 的溶液相比,Cd3(PO4)2 的形成受到鹅绿泥石和桦绿泥石的抑制,这归因于 P 和 Cd 的特定吸附作用,在桦绿泥石中更为明显,因为 Cd 在其空位上的吸附作用更强。所发现的钾和镉的共吸附机制对于理解和预测它们在镉污染环境中的流动性和可用性具有重要意义。
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引用次数: 0
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环境科学与技术
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